Angew. Chem. Int. Ed. | 化学和电化学重构实现协同活性异质结构设计以增强二电子氧还原
时间: 2024-10-07 作者: 浏览次数: 309

题目:

Synergistic Active Heterostructure Design for Enhanced Two Electron Oxygen Reduction via Chemical and Electrochemical Reconstruction of Heterosulfides

作者:

Kai Yu1#, Hongyuan Yang3#, Jie Xu1,4*, Weijie Yuan1, Ruotao Yang1, Meiling Hou5, Zhenhui Kang1*, Yang Liu1, Prashanth W. Menezes2,3* and Ziliang Chen1,2*

摘要:

Transition metal sulfides, particularly heterostructures, represent a promising class of electrocatalysts for two electron oxygen reduction (2e- ORR), however, understanding the dynamic structural evolution of these catalysts during alkaline ORR remains relatively unexplored. Herein, NiS2/In2.77S4 heterostructure was synthesized as a precatalyst and through a series of comprehensive ex situ and in situ characterizations, including X-ray absorption spectroscopy, Raman spectroscopy, transient photo-induced voltage measurements, electron energy loss spectroscopy, and spherical aberration-corrected electron microscopy, it was revealed that nickel/indium (oxy)hydroxides (NiOOH/In(OH)3) could be evolved from the initial NiS2/In2.77S4 via both electrochemical and chemical-driven methods. The electrochemicaldriven phase featured abundant bridging oxygen-deficient [NiO6]-[InO6] units at the interfaces of NiOOH/In(OH)3, facilitating a synergistic effect between active Ni and In sites, thus enabling an enhanced alkaline 2e- ORR capability than that of chemical-driven process. Remarkably, electrochemically induced NiOOH/In(OH)3 exhibited exceptional performance, achieving H2O2 selectivity of >90% across the wide potential window (up to 0.4 V) with a peak selectivity of >99%. Notably, within the three-electrode flow cell, a current density of 200 mA cm-2 was sustained over 20 h, together with an impressive Faradaic efficiency of ~90% during the whole cycle process.

影响因子:

16.1

分区情况:

一区